Merging Platinum Single Atoms to Achieve Ultrahigh Mass Activity and Low Hydrogen Production Cost

Feng Li; Do Hyung Kweon; Gao-Feng Han; Hyuk-Jun Noh; Wei Che; Ishfaq Ahmad; Hu Young Jeong; Zhengping Fu; Yalin Lu; Jong-Beom Baek

doi:10.1021/acsnano.2c11338

Merging Platinum Single Atoms to Achieve Ultrahigh Mass Activity and Low Hydrogen Production Cost

ACS Nano. 2023 Feb 14;17(3):2923-2931. doi: 10.1021/acsnano.2c11338. Epub 2023 Feb 1.

Authors

Feng Li^{1

2}, Do Hyung Kweon², Gao-Feng Han², Hyuk-Jun Noh², Wei Che², Ishfaq Ahmad², Hu Young Jeong³, Zhengping Fu⁴, Yalin Lu⁴, Jong-Beom Baek²

Affiliations

¹ Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 220 Handan, Shanghai 200433, P.R. China.
² School of Energy and Chemical Engineering/Center for Dimension-Controllable Organic Frameworks, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST, Ulsan 44919, South Korea.
³ UNIST Central Research Facilities, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST, Ulsan 44919, South Korea.
⁴ Anhui Laboratory of Advanced Photon Science and Technology, University of Science and Technology of China, 96 Jinzhai, Hefei, Anhui 230026, P.R. China.

PMID: 36722955
DOI: 10.1021/acsnano.2c11338

Abstract

Single atom catalysts (SACs) with isolated active sites exhibit the highest reported mass activity for hydrogen evolution catalysis, which is crucial for practical applications. Here, we demonstrate that ultrahigh mass activity can also be achieved by rationally merging the isolated platinum (Pt) active sites in SAC. The catalyst was obtained by the thermodynamically driven diffusing and merging phosphorus-doped carbon (PC) supported Pt single atoms (Pt₁@PC) into Pt nanoclusters (Pt_M@PC). X-ray absorption spectroscopy analysis revealed that the merged nanoclusters exhibit much stronger interactions with the support than the traditional method, enabling more efficient electron transfer. The optimized Pt_M@PC exhibited an order of magnitude higher mass activity (12.7 A mg_Pt^-1) than Pt₁@PC (0.9 A mg_Pt^-1) at an overpotential of 10 mV in acidic media, which is the highest record to date, far exceeding reports for other outstanding SACs. Theoretical study revealed that the collective active sites in Pt_M@PC exhibit both favorable hydrogen binding energy and fast reaction kinetics, leading to the significantly enhanced mass activity. Despite its low Pt content (2.2 wt %), a low hydrogen production cost of ∼3 USD kg^-1 was finally achieved in the full-water splitting at a laboratory scale.

Keywords: catalyst; electrochemistry; energy conversion; hydrogen evolution reaction; mass activity.